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Angew. Chem. - 日本东北大学Hitoshi Miyasaka教授

发布时间: 2022-4-14 来源: WILEY-VCH

Title: A Host–Guest Electron Transfer Mechanism for Magnetic and Electronic Modifications in a Redox-Active Metal–Organic Framework

Abstract: Host–guest electron transfer (HGET) in molecular framework systems is a critical trigger for drastic functional changes in both host framework and guest. A reversible magnetic phase transition was achieved via HGET in a layered framework, [{Ru2(2,6-F2PhCO2)4}2(BTDA-TCNQ)] (1), where 2,6-F2PhCO2 and BTDA-TCNQ represent 2,6-difluorobenzoate and bis[1,2,5]dithiazolotetracyanoquinodimethane, respectively. The guest-free 1 with an antiferromagnetic ground state transformed into a paramagnet, [{Ru2(2,6-F2PhCO2)4}2(BTDA-TCNQ)]I3 (1-I3), by adsorbing iodine (I2). The local charge distribution of [{Ru2II,III}+-(BTDA-TCNQ).-{Ru2II,II}] in 1 was reversibly modified to [{Ru2II,III}+-(BTDA-TCNQ)0-{Ru2II,II}](I3) in 1-I3 through HGET. Theoretical calculations of 1-I3 indicated a partial charge delocalization as [{Ru2}(1−δ)+-(BTDA-TCNQ)0-{Ru2}δ+](I3) with δ≈0.2, aided by weak ferromagnetic coupling. 1-I3 exhibited a hundred-fold enhancement in electrical conductivity compared to that of 1.

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